Operando single-particle high-resolution Raman imaging of electrocatalysts and batteries
Raj Pandya a, Alexis Grimaud b
a Cavendish Laboratory University of Cambridge, JJ Thomson Avenue, United Kingdom
b Boston College, Department of Chemistry, Boston College, Chestnut Hill, MA, 2467, United States
Materials for Sustainable Development Conference (MATSUS)
Proceedings of Materials for Sustainable Development Conference (MAT-SUS) (NFM22)
#OPCAT - Operando Characterization of Electrocatalytic Interfaces
Barcelona, Spain, 2022 October 24th - 28th
Organizer: Reshma Rao
Invited Speaker, Raj Pandya, presentation 358
DOI: https://doi.org/10.29363/nanoge.nfm.2022.358
Publication date: 11th July 2022

For over 50 years, Raman spectroscopy has remained a key tool in the arsenal of the electrochemists investigating structural and ionic (both solid-state and liquid electrolyte) dynamics in battery and electrocatalytic systems. However, imaging of evolving Raman signals has remained challenging due to the small signals (and hence slow acquisition speeds) of spontaneous Raman. Here, we overcome these limitations and develop and apply high-resolution (sub-300 nm) computational Raman imaging for real-time, chemically specific imaging of operating electrocatalysts and batteries.

Firstly, we track the OER from IrO2 and Li-IrOx electrocatalysts, demonstrating at low overpotentials that oxygen is evolved by the combination of an electrochemical-chemical mechanism and classical electrocatalytic adsorbate mechanism, whereas at high overpotentials only the latter occurs. We then examine electrochemical degradation in LCO and NMC811  electrodes operating at high voltages (above 4.2 V with LP30 electrolyte). For the LCO system, we observe a build-up of degraded electrolyte through the P-F bond intensity and oxidised Co along the edge of the particles.

Our results demonstrate the power of high-resolution Raman microspectroscopy for non-invasive operando, tracking of electrochemical dynamics and reveal new insights into the operation of state-art-of-the-art battery materials and electrocatalysts.



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